DLPNO-MP2 with Periodic Boundary Conditions
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arXiv
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| Autori principali: | , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866915388094152704 |
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| author | Nejad, Arman Zhu, Andrew Sorathia, Kesha Tew, David P. |
| author_facet | Nejad, Arman Zhu, Andrew Sorathia, Kesha Tew, David P. |
| contents | We present domain-based local pair natural orbital Møller--Plesset second order perturbation theory (DLPNO-MP2) with Born--von K{á}rm{á}n boundary (BvK) conditions. The approach is based on well-localised Wannier functions in a LCAO formalism and extends the molecular DLPNO-MP2 implementation Tubromole program package to periodic systems. The PNOs are formed through a PAO-OSV-PNO cascade, using BvK projected atomic orbitals and orbital specific virtuals as intermediaries in an analogous manner to the molecular scheme. Our chargeless and surface-dipole corrected local density fitting approach is shown to be numerically stable and to ensure convergent lattice summations over the periodic images for the two- and three-index Coulomb integrals. Through careful benchmarking, we show that the DLPNO approximations in the BvK-DLPNO-MP2 methods are entirely consistent with those of molecular DLPNO-MP2 calculations, and with an alternative periodic approach Megacell-DLPNO-MP2, reported in Paper II of this series. Smooth convergence to the canonical correlation energy with tightening PNO threshold is observed. Reference MP2 correlation energies are provided for a set of 2D and 3D periodic systems using a triple-zeta basis and supercell sizes up to 11$\times$11 and 7$\times$7$\times$7. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2507_09810 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | DLPNO-MP2 with Periodic Boundary Conditions Nejad, Arman Zhu, Andrew Sorathia, Kesha Tew, David P. Chemical Physics Materials Science Computational Physics We present domain-based local pair natural orbital Møller--Plesset second order perturbation theory (DLPNO-MP2) with Born--von K{á}rm{á}n boundary (BvK) conditions. The approach is based on well-localised Wannier functions in a LCAO formalism and extends the molecular DLPNO-MP2 implementation Tubromole program package to periodic systems. The PNOs are formed through a PAO-OSV-PNO cascade, using BvK projected atomic orbitals and orbital specific virtuals as intermediaries in an analogous manner to the molecular scheme. Our chargeless and surface-dipole corrected local density fitting approach is shown to be numerically stable and to ensure convergent lattice summations over the periodic images for the two- and three-index Coulomb integrals. Through careful benchmarking, we show that the DLPNO approximations in the BvK-DLPNO-MP2 methods are entirely consistent with those of molecular DLPNO-MP2 calculations, and with an alternative periodic approach Megacell-DLPNO-MP2, reported in Paper II of this series. Smooth convergence to the canonical correlation energy with tightening PNO threshold is observed. Reference MP2 correlation energies are provided for a set of 2D and 3D periodic systems using a triple-zeta basis and supercell sizes up to 11$\times$11 and 7$\times$7$\times$7. |
| title | DLPNO-MP2 with Periodic Boundary Conditions |
| topic | Chemical Physics Materials Science Computational Physics |
| url | https://arxiv.org/abs/2507.09810 |